Proposed research program described below represents the extension of efforts initiated over the past two years in the area of synthetic organic chemistry. Our investigations are designed to develop novel and useful methodology for the construction of natural products and related materials having complex, nitrogen containing, polycyclic skeletons. The new methods under development employ ground and excited state initiated molecular rearrangement reactions to elaborate the structural and substitution patterns found in a number of interesting substances belonging to the hydroisoquinoline, and indole alkaloid, mitocene and serratinine families. The focus of our continuing work in this area is the development of new and useful chemistry applicable to the synthesis of naturally occurring and/or medicinally interesting products.